Carbon subsurface traffic jam as driver for methane oxidation activity and selectivity on palladium surfaces
Abstract Separating how surface and subsurface species affect catalytic function is a challenging task in heterogeneous catalysis, particularly when deposition and segregation take place at reaction conditions. Here, we report on an operando approach to establish surface/subsurface/function correlat...
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| Main Authors: | , , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-08-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-63088-9 |
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| _version_ | 1849226154092789760 |
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| author | Ulrike Küst Rosemary Jones Julia Prumbs Alessandro Namar Mattia Scardamaglia Andrey Shavorskiy Jan Knudsen |
| author_facet | Ulrike Küst Rosemary Jones Julia Prumbs Alessandro Namar Mattia Scardamaglia Andrey Shavorskiy Jan Knudsen |
| author_sort | Ulrike Küst |
| collection | DOAJ |
| description | Abstract Separating how surface and subsurface species affect catalytic function is a challenging task in heterogeneous catalysis, particularly when deposition and segregation take place at reaction conditions. Here, we report on an operando approach to establish surface/subsurface/function correlations. Using temperature modulations we oscillate carbon deposition and segregation over a Pd catalyst. Catalytic composition and function are monitored during methane oxidation showing that the surface coverage of carbon drives partial oxidation to CO, while subsurface carbon controls the overall methane turnover. Also, we show that a carbon traffic jam in the subsurface leads to a shifting selectivity from H2 to H2O formation, highlighting the importance of the catalyst subsurface for the catalytic reaction. |
| format | Article |
| id | doaj-art-a69547eefea542e8a62595ce7bd40656 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-08-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-a69547eefea542e8a62595ce7bd406562025-08-24T11:38:20ZengNature PortfolioNature Communications2041-17232025-08-011611710.1038/s41467-025-63088-9Carbon subsurface traffic jam as driver for methane oxidation activity and selectivity on palladium surfacesUlrike Küst0Rosemary Jones1Julia Prumbs2Alessandro Namar3Mattia Scardamaglia4Andrey Shavorskiy5Jan Knudsen6Division of Synchrotron Radiation Research, Lund UniversityDivision of Synchrotron Radiation Research, Lund UniversityDivision of Synchrotron Radiation Research, Lund UniversityPhysics Department, University of TriesteMAX IV Laboratory, Lund UniversityMAX IV Laboratory, Lund UniversityDivision of Synchrotron Radiation Research, Lund UniversityAbstract Separating how surface and subsurface species affect catalytic function is a challenging task in heterogeneous catalysis, particularly when deposition and segregation take place at reaction conditions. Here, we report on an operando approach to establish surface/subsurface/function correlations. Using temperature modulations we oscillate carbon deposition and segregation over a Pd catalyst. Catalytic composition and function are monitored during methane oxidation showing that the surface coverage of carbon drives partial oxidation to CO, while subsurface carbon controls the overall methane turnover. Also, we show that a carbon traffic jam in the subsurface leads to a shifting selectivity from H2 to H2O formation, highlighting the importance of the catalyst subsurface for the catalytic reaction.https://doi.org/10.1038/s41467-025-63088-9 |
| spellingShingle | Ulrike Küst Rosemary Jones Julia Prumbs Alessandro Namar Mattia Scardamaglia Andrey Shavorskiy Jan Knudsen Carbon subsurface traffic jam as driver for methane oxidation activity and selectivity on palladium surfaces Nature Communications |
| title | Carbon subsurface traffic jam as driver for methane oxidation activity and selectivity on palladium surfaces |
| title_full | Carbon subsurface traffic jam as driver for methane oxidation activity and selectivity on palladium surfaces |
| title_fullStr | Carbon subsurface traffic jam as driver for methane oxidation activity and selectivity on palladium surfaces |
| title_full_unstemmed | Carbon subsurface traffic jam as driver for methane oxidation activity and selectivity on palladium surfaces |
| title_short | Carbon subsurface traffic jam as driver for methane oxidation activity and selectivity on palladium surfaces |
| title_sort | carbon subsurface traffic jam as driver for methane oxidation activity and selectivity on palladium surfaces |
| url | https://doi.org/10.1038/s41467-025-63088-9 |
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